epitaxial perovskite oxides on silicon for thermal energy...

Epitaxial perovskite oxides on silicon Epitaxial perovskite oxides on silicon for thermal energy harvesting

R. Bachelet, L. Louahadj, G. Niu, F. Boudaa, J. Penuelas, P. Regreny, B. Vilquin, C. Dubourdieu, M. Gendry, G. Saint-Girons

Institut des Nanotechnologies de Lyon UMR CNRS 5270 http://inl.cnrs.fr

R. Bachelet – GDR Thermoélectricité – Lyon 5 décembre 2012

Context: energy harvesting

• Various sources: Electro-magnetic radiations (solar, RF,..)Mechanical (wind, vibrations,..)Thermal

In nanoscale devices…In nanoscale devices…

• Efficiency / Reliability

• No toxic / Available elements

• Integration• Integration



Thermal energy harvesting

Thermoelectrics (TE) vs Pyroelectrics (PE)

I = f (T) I f (dT/dt)I = f (T) I = f (dT/dt)

Challenges: Challenges:gMaintaining T decreasing sizesDecrease k (by nanostructuring)Twice materials

gSource: T cyclingHarvesting by thermodynamical cyclesLow conversion ratio/Low output power

Low conversion ratio/Low output power Advantage: no need of T

ZT = S2 T/ k



Outline

I N t t d th l t i fil (TE)I. Nanostructured thermoelectric films (TE)

II Possibilities at Institut des Nanotechnologies de Lyon (INL)II. Possibilities at Institut des Nanotechnologies de Lyon (INL)

III. Integrated ABO3 pyroelectric films (PE)3

IV C l iIV. Conclusions



Complex thermoelectrics: nanostructuration

BulkComplex structures reducing thermal conductivity

Clathrates, skutterudites, Half-Heusler,…, , ,Nanostructured composites

nanoclusters in matrix

Thin filmsNanostructured:

Low dimensions structures:Low dimensions structures: 2D: Supperlattices (SLs)1D: Nanowires (NWs)0D: Quantum dots (QDs)( )to scatter phonons=> reduce thermal conductivity

Objectives:ZT > 3

(K < 1 W m-1 K-1) 1

G.J. Snyder et al., Nat. Mat. 7, 105 (2008)



(S > 500 V K-1)y , , ( )

C.J. Vineis et al., Adv. Mat. 22, 3970 (2010)

Nanostructured thermoelectricsI G A i hThin films InGaAs withErAs NPs in SL

With III-Vs materials

InGaAs/InGaAlAs SL

@900 K

J M O Zide et al PRB 74 205335 (2006)



J.M.O. Zide et al., PRB 74, 205335 (2006)W. Kim et al., PRL 96, 045901 (2006)

Nanostructured ABO3 oxide thermoelectricsSrTiO3: a model for oxide electronics

2DEGsO /S O f

SrTiO3: a model for oxide electronics

Tuning (& S)b d i S [2+]Ti[4+]O [2 ] At LaAlO3/SrTiO3 interfaceby doping Sr[2+]Ti[4+]O3

[2-]

Doped by- Aliovalent cations- oxygen vacancies

A. Ohtomo & H.Y. Hwang, Nature 427, 423 (2004)



G. Herranz et al. PRL 98, 216803 (2007)Science 327, 1607 (2010)Nature Materials 11, 91 (2012)

Nanostructured ABO3 oxide thermoelectricsABO filABO3 films:Doped SrTiO3

Nb-STO: Sr[2+](Ti[4+],Nb[5+])O3

[2-]

La-STO:(La[3+],Sr[2+])Ti[4+]O3

[2-]

T = 300 K

H Ohta et al Nat Mat 6 129 (2007)B. Jalan and S. Stemmer,



H. Ohta et al., Nat. Mat. 6, 129 (2007)S. Ohta et al., APL 87, 092108 (2005)

B. Jalan and S. Stemmer, APL 97, 042106 (2010)

Institut des Nanotechnologies de Lyon (INL)

•Biotechnologies et Santé

4 départements Personnel22 CR & DR CNRS71 MCF & Prof.

•Photonique / Photovoltaïque•Matériaux Fonctionnels•Electronique

71 MCF & Prof.44 ITA115 Docs & post-docs

9 équipes

4 sites INSA

•Hétéroépitaxie et Nanostructures•Spectroscopie et NanomatériauxDispositifs Electroniques

9 équipesECLUCBLCPE

•Dispositifs Electroniques•Heterogeneous Systems Design•Nanophotonique•Photovoltaïque•Photovoltaïque•Chimie et Nanobiotechnologies•Microfluidique - Microsystèmes•Capteurs Biomédicaux



Capteurs Biomédicaux

INL: team H&N + NanoLyon platform

Team H&N: « Heteroepitaxy and Nanostructures »Head: Michel Gendry & Guillaume Saint-Girons

3 MBE chambers + XPS in a new clean room



3 MBE chambers + XPS in a new clean roomCoupled in line: III-V MBE + oxide MBE + XPS

(contact: Philippe Regreny)

III-Vs nanostructuresSemiconductor nanostructures: reducing dimensionsSemiconductor nanostructures: reducing dimensions…

2D: SLs & QWs 1D: NWs InP

200 nmInAlAsP

0D: QDs0D: QDs



Works led by Michel Gendry, H&N team, INL

Integrated ABO3 nanostructuresEpitaxial SrTiO3/SiEpitaxial SrTiO3/Si…

14 ML

STO(110)1000 2)) STO(110)

(a) 100 W

100

1000

cps)

SrTiO2.5Si(0

04)

SrT

iO3(

002

SrT

iO3(

001)

.)

(b) 200 W

20 30 40 50 60 70

10

Int.

(c

nsity

(a.u

.

(c) 300 W

20 30 40 50 60 70

2 (°)

Inte

(d) 400 W SrTiO

0 34 0 35 0 36 0 37 0 38

SrTiO3



0,34 0,35 0,36 0,37 0,38

q// (Å-1)G. Niu et al. APL 2009 L. Laouhadj et al.

Integrated ABO3 nanostructuresEpitaxial ABO3/SrTiO3/SiEpitaxial ABO3/SrTiO3/Si…

Ferroelectric ABO3

LAO/STO SLs

P

LaAlO3

SrTiO3

LaAlO3

SrTiO3

4 nm4 nmO. Marty ‐ INL(UCBL)

C. Merckling et al.G Niu et al Thin Sol Films 520 4595 (2012)



G. Niu et al., Thin Sol. Films 520, 4595 (2012)G. Niu et al., Microelec. Eng. 88, 1232 (2011)

Pyroelectrics (PE)

Diél t i • InsulatorsSrTiO

Similar ABO3 Many applicationsO. Auciello et al. Phys. Today (1998)

Diélectriques

Piezo

• Insulators

• ActuatorsPb(Zr,Ti)O3

SrTiO3

Ferro

Pyro • Sensors

•MemoriesBaTiO3

(Ba,Sr)TiO3

Ferro Memories3

P



Pyroelectrics (PE)

20°C peak-peakHarvesting by thermodynamical cycles

G S b ld t l S t M t St t 18

Heat exchange

G. Sebald et al., Smart Mater. Struct. 18, 125006 (2009)

G. Sebald et al., IEEE Transac. Ultrason.

Increasing outputs by:- non linear effects- SSH methods



G. Sebald et al., IEEE Transac. Ultrason. Ferroelec. Freq. Control 55, 538 (2008)D. Guyomar et al., LGEF

Integrated pyroelectrics (PE)FE/SOIFE/SOI

US patent US2012056504, «MEMS-based pyroelectric Thermal Energy Harvester» by S R Hunter et al Oak Ridge (2010)



by S.R. Hunter et al., Oak Ridge (2010)

Conclusions/Perspectives

TE epitaxial films: - Nanostructuring!Nanostructuring!SLs (with 2DEGs)nanocomposites: NWs in matrix (core/shell) ?...

- Epitaxy of new phases?..

- Open for collaborations!..

PE epitaxial films:- Possible energy harvesters with reduced sizes- Possible energy harvesters with reduced sizes- Enhancing conversion with strained epitaxial films?...



epitaxial perovskite oxides on silicon for thermal energy...

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